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Highlights and News at MBI
Earlier Highlights are found in the archive
24th March 2015: Classical or not? Physics of nanoplasmas
The interaction of an intense laser pulse with a nanometer-scale particle results in the generation of an expanding nanoplasma. In the past, nanoplasma dynamics were typically described by classical phenomena, like the thermal emission of electrons. In contrast, a new study on the interaction of intense near-infrared (NIR) laser pulses with molecular oxygen clusters now demonstrates that phenomena, which can only be described quantummechanically, play an important role. ... more.
 
11th February 2015: New Insights into the photophysics of the DNA base thymin
DNA stores our genetic code. Solar UV radiation has sufficiently high energy to basically break bonds of the DNA and thus cause DNA damage. Although DNA (e. g. in our skin cells) is exposed to intense UV light irradiation, DNA proves to be surprising photostable. ... more.
 
10th February 2015: Nonlinear resonance disaster in the light of ultrashort pulses
Ultrashort light pulses from modern lasers enable temporal resolution of even the fastest processes in molecules or solid-state materials. ... more.
 

 
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Classical or not? Physics of nanoplasmas


24. March 2015

The interaction of an intense laser pulse with a nanometer-scale particle results in the generation of an expanding nanoplasma. In the past, nanoplasma dynamics were typically described by classical phenomena, like the thermal emission of electrons. In contrast, a new study on the interaction of intense near-infrared (NIR) laser pulses with molecular oxygen clusters now demonstrates that phenomena, which can only be described quantummechanically, play an important role. For the first time, evidence of efficient formation of autoionizing states in nanoplasmas is found. Autoionization of so called superexcited states of atomic oxygen is directly observed on a nanosecond time scale, whereas indirect signatures are visible for decay processes occurring on shorter time scales. Autoionization is found to take place in various systems and is expected to be important also in the interaction of finite systems with intense extreme-ultraviolet (XUV) and X-ray pulses from novel free-electron laser sources.

Following the interaction of intense NIR laser pulses with clusters, the recorded electron spectra typically show a smooth distribution. In the past, the absence of discrete state signatures in these spectra led to the conclusion that the dynamics of charged particles during the cluster expansion can be well described by fully classical behavior. As a consequence, simulations that model the interaction of intense lasers with clusters, nanoparticles or large molecules, often make use of quasiclassical approaches. With the advent of novel laser sources and time-resolved techniques during the last year, this picture began to falter. Recently, extensive formation of excited atoms in nanoplasmas driven by electron-ion recombination processes was reported. When an atom with 2 electrons in excited states is formed, it may decay via an electron correlation effect, where one electron is released into the continuum, while the second electron relaxes to a lower bound state. However, since the electrons emitted via such autoionization processes exchange kinetic energy with the cluster environment, they had not been observed in experiments so far.

In a collaboration led by scientists from the Max-Born-Institut, the first evidence of autoionization following intense NIR laser-cluster interactions is now reported. In the current issues of Physical Review Letters [114, 123002 (2015)] Bernd Sch├╝tte, Marc Vrakking and Arnaud Rouz├ęe, and their colleagues Jan Lahl, Tim Oelze and Maria Krikunova from the TU Berlin present results obtained from oxygen clusters. This system was chosen, because oxygen atoms have previously been shown to exhibit long-lived autoionizing states. In the present study, clear peaks were observed in the electron spectrum from oxygen clusters ionized by intense NIR pulses (Fig. 1). These peaks could be assigned to well-known autoionizing states, and it was shown that they decay on a nanosecond time scale, when the cluster has already significantly expanded. Therefore, the influence of the environment on the electrons emitted via autoionization was negligible. The observed autoionization contributions were found to be very sensitive on the intensity of the NIR laser pulse. At higher intensities, the autoionization peaks were blurred out, but still visible. These results indicate that autoionization plays an important role in many experiments that study the interaction of intense laser pulses with nanometer-scale systems, even when these processes cannot be directly observed in the electron spectrum. Previously, it was demonstrated that the observed nanoplasma dynamics following intense XUV and NIR ionization of clusters are similar, and therefore, the current results are expected to be highly relevant as well for experiments at novel free-electron lasers. The experimental findings of autoionization are also important for improving theoretical models of nanoplasmas in the future in order to gain a better understanding of the underlying microscopic processes.

The presented results demonstrate that a description of nanoplasma dynamics by classical approaches is insufficient. Quantum phenomena like autoionization play an important role during the expansion of clusters following the interaction with intense light pulses.

Originalpublication: Physical Review Letters

Full citation:

Bernd Schütte, Jan Lahl, Tim Oelze, Maria Krikunova, Marc J. J. Vrakking and Arnaud Rouzée, "Efficient autoionization following intense laser-cluster interactions", Physical Review Letters 114, 123002 (2015)

doi: http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.114.123002

Contact:

Dr. Bernd Schütte

Prof. Marc J. J. Vrakking

Dr. Arnaud Rouzée

schuette2015

Fig. 1: (a) Two-dimensional electron momentum map emitted from O2 molecules, showing an anisotropic distribution of electrons peaked along (vertical)  the NIR laser polarization. (b) In the corresponding kinetic energy spectrum, the observed peaks are attributed to above-threshold ionization and Freeman resonances. (c) The electron momentum map from O2 clusters with an average size of 2400 molecules exhibits a much more isotropic behavior. (d) In the kinetic energy spectrum, three clear peaks emerge that are assigned to autoionization of superexcited atomic states.

 

Fig. 1  
 
     
 


New Insights into the photophysics of the DNA base thymine


11th February 2015

DNA stores our genetic code. Solar UV radiation has sufficiently high energy to basically break bonds of the DNA and thus cause DNA damage. Although DNA (e. g. in our skin cells) is exposed to intense UV light irradiation, DNA proves to be surprising photostable. It is well established that this is due to efficient mechanisms that convert electronic energy into other forms of energy, in particular heat. An important role is played by so-called conical intersections between electronic excited potential energy surfaces and the ground state potential energy surface. These conical intersections are associated with structural changes of the molecules. The exact pathways back into the electronic ground state however are topic of intense research.

Although DNA is a macro molecule with billions of atoms (in case of human DNA), it can still be divided into only a few structural (and functional) elements: four DNA bases, a sugar moiety and a phosphate group. The absorption of UV light exclusively takes place in the DNA bases. For this reason it is a common scientific approach to investigate the UV response of DNA bases, first.

A team of scientists from MBI and universities of Hokkaido and Hirosaki in Japan have for the first time investigated the DNA base thymine in aqueous solution by time-resolved photoelectron spectroscopy and questioned existing ideas about the excited-state relaxation process in this base. So far was supposed that a significant fraction of the excited-state population remains in a dark nπ* state instead of immediately returning to the ground state via a conical intersection. This dark state cannot be observed by optical spectroscopy (e. g. transient absorption or fluorescence upconversion), directly. Corresponding limitations however do not exist for photoelectron spectroscopy.

By combining experiment and simulation, for the first time two different relaxation pathways were identified. Both pathes evolve in the first excited state (ππ*). The faster reaction path is associated with a twist of the aromatic ring and leads to repopulation of the electronic ground state within 100 fs. The second path involves an out-of-plane motion of the carbonyl group, and the molecule returns to the ground state within 400 fs. The scientists did not find any indication for an important role of the second excited nπ* state and conclude that this state is not involved in the relaxation process.

Original publication:
Franziska Buchner, Akira Nakayama, Shohei Yamazaki, Hans-Hermann Ritze, Andrea Lübcke
Excited-State relaxation of hydrated thymine and thymidine measured by liquid-jet photoelectron spectroscopy: experiment and simulation, JACS,
JACS, DOI: 10.1021/ja511108u

folgt in K├╝rze

Fig. 1: After UV excitation thymine evolves on the (ππ*) excited state surface along two different reaction coordinates. The first involves a twisting of the aromatic ring, the second an out-of-plane motion of the carbonyl group. In contrast to existing ideas, the nπ* state does not seem to be involved in the relaxation process..

Fig. 1 (click to enlarge)


Contact:
Dr. Andrea Lübcke Tel: 030 6392 1207



 
     
 

Nonlinear resonance disaster in the light of ultrashort pulses


10th February 2015

Ultrashort light pulses from modern lasers enable temporal resolution of even the fastest processes in molecules or solid-state materials. For example, chemical reactions can, in principle, be traced down to the 10-fs time scale (1 femtosecond (fs) = 10-15 s). Ten femtoseconds correspond to a few oscillation cycles of the light field itself. Nevertheless, there is a class of optical processes that does not exhibit any measurable delay relative to the ultrafast light oscillation and which has been termed “instantaneous”. This class of processes includes nonlinear optical harmonic generation at multiple frequencies of the input field. This process is commonly used to generate the green light of laser pointers from invisible infrared light. These processes are normally used far away from a resonance to avoid losses.

In a collaborative effort, researchers of the Max-Born-Institut, the Weierstraß-Institut as well as the Leibniz-Universität Hannover now experimentally demonstrated for the first time that conditions exist where optical harmonic generation becomes non-instantaneous. Analyzing third-harmonic generation in titanium dioxide thin films, a lifetime of 8 fs was found, i.e., non-instantaneous behavior. Nevertheless, this process still qualifies as one of the fastest processes ever resolved with femtosecond spectroscopy.

Detailed theoretical modeling of these surprising findings indicates that this non-instantaneous response may only occur if there is a resonance of the third harmonic in the optical material. In turn, the generated material response persists to oscillate several cycles after the excitation has already ceased. Concomitantly, third-harmonic radiation is emitted. The process therefore appears like an atomic “resonance disaster”. Similar to mechanical oscillators, this atomic system therefore shows a non-instantaneous behavior.

These findings have important consequences for femtosecond measurement techniques and possibly also for ultrashort-pulse generation. These methods have always relied on an instantaneous nature of harmonic generation and related effects. Similar to soldiers who avoid marching in step on a suspension bridge, one therefore also has to carefully avoid optical resonances when measuring extremely short laser pulses.

Original publication:
Michael Hofmann, Janne Hyyti, Simon Birkholz, Martin Bock, Susanta K. Das, Rüdiger Grunwald, Mathias Hoffmann, Tamas Nagy, Ayhan Demircan, Marco Jupé, Detlev Ristau, Uwe Morgner, Carsten Brée, Michael Woerner, Thomas Elsaesser, Guenter Steinmeyer
Noninstantaneous polarization dynamics in dielectric media
OPTICA doi.org/10.1364/OPTICA.2.000151

 

ResponseJPG

Figure 1: Reaction of SiO2 and TiO2 to a short pulsed light field. In SiO2 the displacement of electron shell follows the exciting electric field. Immediately after the end of the pulse, this oscillation ceases, too. In contrast, in TiO2, an oscillation build-up is observed at the third harmonic of the exciting field. This oscillation continues beyond the end of the pulse. Insets show pictures of crystalline modifications for both optical materials (Photographs by Didier Descouens, CC BY 3.0 and Rob Lavinsky, CC-BY-SA-3.0).

Fig. 1 (click to enlarge)

visualize4

Movie: Reaction of SiO2 and TiO2 to a short pulsed light field. The electric field is visualized by the central arrow. The resulting displacement of the electron shell is shown in a simple atomic picture for both materials. Third-harmonic emission is indicated by a blue color of the shell. In SiO2, both the resulting oscillation as well as the harmonic emission immediately cease after the end of the exciting pulse. In contrast, TiO2 exhibits a resonant build-up of the third-harmonic oscillation, which persists beyond the duration of the exciting pulse.

Fig. 2 (click for animation - AVI-file)  


Contact
Dr. Günter Steinmeyer Tel: 030 6392 1440

 
     



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